Magnetic anisotropy and spin-polarized two-dimensional electron gas in the van der Waals ferromagnet Cr₂Ge₂Te₆

We report a comprehensive experimental investigation on the magnetic anisotropy in bulk single crystals of Cr$_2$Ge$_2$Te$_6$, a quasi-two-dimensional ferromagnet belonging to the family of magnetic layered transition metal trichalcogenides that have attracted recently a big deal of interest with regard to the fundamental and applied aspects of two-dimensional magnetism. For this purpose electron spin resonance (ESR) and ferromagnetic resonance (FMR) measurements have been carried out over a wide frequency and temperature range. A gradual change in the angular dependence of the ESR linewidth at temperatures above the ferromagnetic transition temperature $T_{\rm c}$ reveals the development of two-dimensional spin correlations in the vicinity of $T_{\rm c}$ thereby proving the intrinsically low-dimensional character of spin dynamics in Cr$_2$Ge$_2$Te$_6$. Angular and frequency dependent measurements in the ferromagnetic phase clearly show an easy-axis type anisotropy of this compound. Furthermore, these experiments are compared with simulations based on a phenomenological approach, which takes into account results of static magnetization measurements as well as high temperature $g$ factors obtained from ESR spectroscopy in the paramagnetic phase. As a result the determined magnetocrystalline anisotropy energy density (MAE) $K_U$ is $(0.48 \pm 0.02) \times10^6$ erg/cm$^3$. This analysis is complemented by density functional calculations which yield the experimental MAE value for a particular value of the electronic correlation strength $U$. The analysis of the electronic structure reveals that the low-lying conduction band carries almost completely spin-polarized, quasi-homogeneous, two-dimensional states.